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BiSe is found to be a promising near-room-temperature thermoelectric material with higher performance than traditional Bi2Se3 due to its ultra-low intrinsic lattice thermal conductivity. In this work, N-type BiSe nanocrystalline thin films with (00l) preferred orientation are first prepared via vacuum thermal evaporation method, and Bi1–xSbxSe nanocrystalline films with different doping concentrations are obtained by Sb co-evaporation. The phases, morphologies, chemical compositions and valences, lattical vibrations, and electrical properties of these films are characterized. It is found that the Sb dopant successfully enters into the crystal lattice and replaces the Bi site of Bi2Se3 quintuple layers and Bi2 bilayers without selectivity, and the difference of gold properties between Sb atom and Bi atoms leads the carrier concentration to sharply decrease and the Seebeck coefficient in doped BiSe to increase. Meanwhile, the sizes of nanocrystals in the films decrease and the denser layered structure is formed due to the Sb doping, which is conducive to the carrier transport in the samples, and the in-plane carrier mobility of the films effectively increases from 13.6 cm2·V–1·s–1 (BiSe) to 19.3 cm2·V–1·s–1 (Bi0.65Sb0.35Se). The maximum room-temperature power factor of 2.18 μW·cm–1·K–2 is obtained in Bi0.76Sb0.24Se, which is higher than that in undoped BiSe. The results of this work indicate that the BiSe-based thin films have potential applications in room temperature thermoelectric thin film devices. -
Keywords:
- N-type /
- Bi1–xSbxSe /
- thermoelectric nanocrystalline films /
- layered structure /
- power factor
[1] Zhou M, Al-Furjan M S H, Zou J, Liu W 2018 Renew. Sust. Energ. Rev. 82 3582Google Scholar
[2] Kraemer D, Jie Q, McEnaney K, Cao F, Liu W, Weinstein L A, Loomis J, Ren Z, Chen G 2016 Nat. Energy 1 16153Google Scholar
[3] Hasan M N, Wahid H, Nayan N, Mohamed Ali M S 2020 Int. J. Energy Res. 44 6170Google Scholar
[4] Chen A, Madan D, Wright P K, Evans J W 2011 J. Micromech. Microeng. 21 104006Google Scholar
[5] Orr B, Akbarzadeh A, Mochizuki M, Singh R 2016 Appl. Therm. Eng. 101 490Google Scholar
[6] Lee K H, Kim S W 2017 J. Korean Ceram. Soc. 54 75Google Scholar
[7] Samanta M, Pal K, Pal P, Waghmare U V, Biswas K 2018 J. Am. Chem. Soc. 140 5866Google Scholar
[8] Lind H, Lidin S, Häussermann U 2005 Phys. Rev. B. 72 184101Google Scholar
[9] Ju Z, Hou Y, Bernard A, Taufour V, Yu D, Kauzlarich S M 2019 CS Appl. Electron. 1 1917
[10] Samanta M, Biswas K 2020 Chem. Mater. 32 8819Google Scholar
[11] Zhang J, Huang G 2014 Solid State Commun. 197 34Google Scholar
[12] Valla T, Ji H, Schoop L, Weber A, Pan Z-H, Sadowski J, Vescovo E, Fedorov A, Caruso A, Gibson Q 2012 Phys. Rev. B. 86 241101Google Scholar
[13] Ouyang Y, Zhang Z W, Li D F, Chen J, Zhang G 2019 Ann. Phys. (Berlin) 531 1800437Google Scholar
[14] Qiu B, Ruan X L 2009 Phys. Rev. B 80 165203Google Scholar
[15] He J, Hu X X, Li D F, Chen J 2022 Nano Res. 15 3804Google Scholar
[16] Shen X C, Zhang X, Zhang B, Wang G Y, He J, Zhou X Y 2020 Rare Metals 39 1374Google Scholar
[17] He Z M, Lan K L, Chen S Y, Dong Y Z, Lai X F, Liu F S, Jian J K 2022 J. Alloys Compd. 901 163652Google Scholar
[18] Shi X L, Zou J, Chen Z G 2020 Chem. Rev. 120 7399Google Scholar
[19] 魏江涛, 杨亮亮, 秦源浩, 宋培帅, 张明亮, 杨富华, 王晓东 2021 70 047301Google Scholar
Wei J T, Yang L L, Qin Y H, Song P S, Zhang M L, Yang F H, Wang X D 2021 Acta Phys. Sin. 70 047301Google Scholar
[20] Venkatasubramanian R, Siivola E, Colpitts T, O'Quinn B 2001 Nature 413 597Google Scholar
[21] Li J F, Liu W S, Zhao L D, Zhou M 2010 NPG Asia Mater. 2 152Google Scholar
[22] Wu H, Carrete J, Zhang Z, Qu Y, Shen X, Wang Z, Zhao L-D, He J 2014 NPG Asia Mater. 6 e108Google Scholar
[23] Dun C, Hewitt C A, Huang H, Xu J, Zhou C, Huang W, Cui Y, Zhou W, Jiang Q, Carroll D L 2015 Nano Energy 18 306Google Scholar
[24] 陈赟斐, 魏锋, 王赫, 赵未昀, 邓元 2021 70 207303Google Scholar
Chen Y F, Wei F, Wang H, Zhao W Y, Deng Y 2021 Acta Phys. Sin. 70 207303Google Scholar
[25] Adam A M, El-Khouly A, Diab A K 2021 J. Alloys Compd. 851 156887Google Scholar
[26] Lu M P, Liao C N, Huang J Y, Hsu H C 2015 Inorg. Chem. 54 7438Google Scholar
[27] Kim K, Kim G, Kim S I, Lee K H, Lee W 2019 J. Alloys Compd. 772 593Google Scholar
[28] Chen C L, Wang H, Chen Y Y, Day T, Snyder G J 2014 J. Mater. Chem. A. 2 11171Google Scholar
[29] Han M K, Hoang K, Kong H, Pcionek R, Uher C, Paraskevopoulos K M, Mahanti S D, Kanatzidis M G 2008 Chem. Mater. 20 3512Google Scholar
[30] Ibrahim E M M, Hakeem A M A, Adam A M M, Shokr E K 2015 Phys. Scr. 90 045802Google Scholar
[31] Bando H, Koizumi K, Oikawa Y, Daikohara K, Kulbachinskii V A, Ozaki H 2000 J. Phys. Condens. Matter 12 5607Google Scholar
[32] Jia F, Liu Y Y, Zhang Y F, Shu X, Chen L, Wu L M 2020 J. Am. Chem. Soc. 142 12536Google Scholar
[33] Liu X, Chen J, Luo M, Leng M, Xia Z, Zhou Y, Qin S, Xue D J, Lv L, Huang H, Niu D, Tang J 2014 ACS Appl. Mater. Interfaces 6 10687Google Scholar
[34] Zhang C, Yin H, Han M, Dai Z, Pang H, Zheng Y, Lan Y Q, Bao J, Zhu J 2014 ACS Nano 8 3761Google Scholar
[35] Heremans J P, Jovovic V, Toberer E S, Saramat A, Kurosaki K, Charoenphakdee A, Yamanaka S, Snyder G J 2008 Science 321 554Google Scholar
[36] Jia B, Liu S, Li G, Liu S, Zhou Y, Wang Q 2019 Thin Solid Films 672 133Google Scholar
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图 6 Bi1–xSbxSe纳米晶薄膜(x = 0, 0.15, 0.24, 0.35)在不同温度下的 (a) 载流子浓度; (b) 迁移率; (c) 面内电导率; (d) 塞贝克系数; (e) 功率因子
Figure 6. Temperature dependence of (a) carrier concentrations, (b) electron mobilities, (c) the in-plane conductivities, (d) Seebeck coefficients and (e) power factors for Bi1–xSbxSe (x = 0, 0.15, 0.24, 0.35) samples.
表 1 Bi1–xSbxSe纳米薄膜的实验条件
Table 1. Experimental conditions of Bi1–xSbxSe thin films.
样品 (Bi+Bi2Se3)蒸发源温度/℃ Sb蒸发源温度/℃ 源与衬底的距离/cm 衬底温度/
℃蒸镀时间/
minBiSe 500 — 10 475 10 Bi0.85Sb0.15Se 500 300 10 475 10 Bi0.76Sb0.24Se 500 350 10 475 10 Bi0.65Sb0.35Se 500 375 10 475 10 表 2 Bi1–xSbxSe薄膜的元素原子比
Table 2. Atomic ratio of Bi1–xSbxSe thin films.
样品 Bi/% Sb/% Se/% BiSe 49.97 — 50.03 Bi0.85Sb0.15Se 42.37 7.53 50.10 Bi0.76Sb0.24Se 38.01 11.91 50.08 Bi0.65Sb0.35Se 32.49 17.45 50.05 表 3 Bi1–xSbxSe (x = 0, 0.15, 0.24, 0.35)薄膜的拉曼振动峰(cm–1)
Table 3. Raman vibration peaks (cm–1) of Bi1–x SbxSe (x = 0, 0.15, 0.24, 0.35) films.
BiSe Bi0.85Sb0.15Se Bi0.76Sb0.24Se Bi0.65Sb0.35Se $ \rm A^1_{1g} $ 68.1 70.5 70.9 71.4 Eg 93.7 95.4 95.9 96.7 $ \rm E^2_g $ 120.6 121.4 122.1 122.9 $\rm A^2_{1g}$ 155.4 157.9 160.5 161.5 表 4 Bi1–xSbxSe(x = 0, 0.15, 0.24, 0.35)薄膜在室温下的霍尔效应测试结果
Table 4. The electrical transport properties of Bi1–xSbxSe (x = 0, 0.15, 0.24, 0.35) thin films at room temperature.
薄膜样品 载流子浓度
n/(1020 cm–3)载流子迁移率
μ/(cm2·V–1·s–1)电导率
σ/(S·cm–1)BiSe 2.5 13.6 544.2 Bi0.85Sb0.15Se 1.9 16.7 502.3 Bi0.76Sb0.24Se 1.6 18.4 468.8 Bi0.65Sb0.35Se 1.3 19.3 416.8 -
[1] Zhou M, Al-Furjan M S H, Zou J, Liu W 2018 Renew. Sust. Energ. Rev. 82 3582Google Scholar
[2] Kraemer D, Jie Q, McEnaney K, Cao F, Liu W, Weinstein L A, Loomis J, Ren Z, Chen G 2016 Nat. Energy 1 16153Google Scholar
[3] Hasan M N, Wahid H, Nayan N, Mohamed Ali M S 2020 Int. J. Energy Res. 44 6170Google Scholar
[4] Chen A, Madan D, Wright P K, Evans J W 2011 J. Micromech. Microeng. 21 104006Google Scholar
[5] Orr B, Akbarzadeh A, Mochizuki M, Singh R 2016 Appl. Therm. Eng. 101 490Google Scholar
[6] Lee K H, Kim S W 2017 J. Korean Ceram. Soc. 54 75Google Scholar
[7] Samanta M, Pal K, Pal P, Waghmare U V, Biswas K 2018 J. Am. Chem. Soc. 140 5866Google Scholar
[8] Lind H, Lidin S, Häussermann U 2005 Phys. Rev. B. 72 184101Google Scholar
[9] Ju Z, Hou Y, Bernard A, Taufour V, Yu D, Kauzlarich S M 2019 CS Appl. Electron. 1 1917
[10] Samanta M, Biswas K 2020 Chem. Mater. 32 8819Google Scholar
[11] Zhang J, Huang G 2014 Solid State Commun. 197 34Google Scholar
[12] Valla T, Ji H, Schoop L, Weber A, Pan Z-H, Sadowski J, Vescovo E, Fedorov A, Caruso A, Gibson Q 2012 Phys. Rev. B. 86 241101Google Scholar
[13] Ouyang Y, Zhang Z W, Li D F, Chen J, Zhang G 2019 Ann. Phys. (Berlin) 531 1800437Google Scholar
[14] Qiu B, Ruan X L 2009 Phys. Rev. B 80 165203Google Scholar
[15] He J, Hu X X, Li D F, Chen J 2022 Nano Res. 15 3804Google Scholar
[16] Shen X C, Zhang X, Zhang B, Wang G Y, He J, Zhou X Y 2020 Rare Metals 39 1374Google Scholar
[17] He Z M, Lan K L, Chen S Y, Dong Y Z, Lai X F, Liu F S, Jian J K 2022 J. Alloys Compd. 901 163652Google Scholar
[18] Shi X L, Zou J, Chen Z G 2020 Chem. Rev. 120 7399Google Scholar
[19] 魏江涛, 杨亮亮, 秦源浩, 宋培帅, 张明亮, 杨富华, 王晓东 2021 70 047301Google Scholar
Wei J T, Yang L L, Qin Y H, Song P S, Zhang M L, Yang F H, Wang X D 2021 Acta Phys. Sin. 70 047301Google Scholar
[20] Venkatasubramanian R, Siivola E, Colpitts T, O'Quinn B 2001 Nature 413 597Google Scholar
[21] Li J F, Liu W S, Zhao L D, Zhou M 2010 NPG Asia Mater. 2 152Google Scholar
[22] Wu H, Carrete J, Zhang Z, Qu Y, Shen X, Wang Z, Zhao L-D, He J 2014 NPG Asia Mater. 6 e108Google Scholar
[23] Dun C, Hewitt C A, Huang H, Xu J, Zhou C, Huang W, Cui Y, Zhou W, Jiang Q, Carroll D L 2015 Nano Energy 18 306Google Scholar
[24] 陈赟斐, 魏锋, 王赫, 赵未昀, 邓元 2021 70 207303Google Scholar
Chen Y F, Wei F, Wang H, Zhao W Y, Deng Y 2021 Acta Phys. Sin. 70 207303Google Scholar
[25] Adam A M, El-Khouly A, Diab A K 2021 J. Alloys Compd. 851 156887Google Scholar
[26] Lu M P, Liao C N, Huang J Y, Hsu H C 2015 Inorg. Chem. 54 7438Google Scholar
[27] Kim K, Kim G, Kim S I, Lee K H, Lee W 2019 J. Alloys Compd. 772 593Google Scholar
[28] Chen C L, Wang H, Chen Y Y, Day T, Snyder G J 2014 J. Mater. Chem. A. 2 11171Google Scholar
[29] Han M K, Hoang K, Kong H, Pcionek R, Uher C, Paraskevopoulos K M, Mahanti S D, Kanatzidis M G 2008 Chem. Mater. 20 3512Google Scholar
[30] Ibrahim E M M, Hakeem A M A, Adam A M M, Shokr E K 2015 Phys. Scr. 90 045802Google Scholar
[31] Bando H, Koizumi K, Oikawa Y, Daikohara K, Kulbachinskii V A, Ozaki H 2000 J. Phys. Condens. Matter 12 5607Google Scholar
[32] Jia F, Liu Y Y, Zhang Y F, Shu X, Chen L, Wu L M 2020 J. Am. Chem. Soc. 142 12536Google Scholar
[33] Liu X, Chen J, Luo M, Leng M, Xia Z, Zhou Y, Qin S, Xue D J, Lv L, Huang H, Niu D, Tang J 2014 ACS Appl. Mater. Interfaces 6 10687Google Scholar
[34] Zhang C, Yin H, Han M, Dai Z, Pang H, Zheng Y, Lan Y Q, Bao J, Zhu J 2014 ACS Nano 8 3761Google Scholar
[35] Heremans J P, Jovovic V, Toberer E S, Saramat A, Kurosaki K, Charoenphakdee A, Yamanaka S, Snyder G J 2008 Science 321 554Google Scholar
[36] Jia B, Liu S, Li G, Liu S, Zhou Y, Wang Q 2019 Thin Solid Films 672 133Google Scholar
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